Freezing by heating in a driven mesoscopic system

We investigate a simple model corresponding to particles driven in opposite directions and interacting via a repulsive potential. The particles move off-lattice on a periodic strip and are subject to random forces as well. We show that this model-which can be considered as a continuum version of some driven diffusive systems-exhibits a paradoxical, new kind of transition called here "freezing by heating." One interesting feature of this transition is that a crystallized state with a higher total energy is obtained from a fluid state by increasing the amount of fluctuations.     

Size dependence of freezing temperature and structure instability in simulated Lennard-Jones clusters

Liquid Lennard-Jones clusters of 14 different sizes from N=55 to 923 particles were cooled down to find their temperature of liquid-solid transition and the internal structure of the solidified clusters. The decrease of the cluster temperature was attained by a gradual change of the system temperature in Monte Carlo simulations. The liquid-to-solid transition was found by analysis of the specific heat as well as by detection of the structural units of face-centred cubic, hexagonal close-packed and decahedral type. It was observed that near the detected transition temperature the solid-like cluster structure is not always stable and fluctuates between solid and liquid states. The fluctuations of the state were observed frequently for small clusters with N ≤147, where the temporary solid structure is created by a large part of internal atoms. Manual inspection of cluster structural data and the 10%N condition for minimal number of atoms as centres of solid-like units enable detection of stable cluster solidification at freezing temperature. It was found that the freezing temperature of all clusters, with the exception of N=55, decreases linearly with N^-1/3. The extrapolated freezing temperature of the bulk LJ system is 13% lower than the experimental value of argon. After freezing, the solid phase remains but some atoms close to the cluster surface are not firmly included into the structure and oscillate mainly between solid structure and disordered one.     

静电场对红细胞悬液冻结特性的影响

本文以红细胞悬液为研究模型,通过在对其进行慢速冻结的过程中引入静电场,具体研究了静电场对降温过程中红细胞悬液冻结特性的影响。实验结果表明:静电场在一定程度上改变了冰晶的形成与生长特性,抑制了晶核的形成, 使晶枝出现不对称生长,并减缓了冰晶的生长速度,这些影响随着场强的增加而逐渐加强。在较强的静电场的影响下,冰晶明显变粗,最终成为块状,细胞也不再与冰晶分离而是完全融入粗大的冰晶之中,在冻结的末期,细胞不再受到冰晶挤压,从而减少了其所受的机械性损伤。     

Nonequilibrium phase transition in the sedimentation of reproducing particles

We study numerically and analytically the dynamics of a sedimenting suspension of active, reproducing particles, such as growing bacteria in a gravitational field. In steady state we find a nonequilibrium phase transition between a "sedimentation" regime, analogous to the sedimentation equilibrium of passive colloids, and a "uniform" regime, in which the particle density is constant in all but the top and bottom of the sample. We discuss the importance of fluctuations in particle density in locating the phase-transition point, and report the kinetics of sedimentation at early times.     

Continuous freezing in three dimensions

We analyze the freezing transition in a system of hard particles with a very long-ranged repulsion. The long-range repulsion makes first-order freezing transitions continuous, but leaves the initial stages of the crystallization unchanged: the crystal phase must still nucleate. The coexistence between bulk phases is replaced by microphase separation.     

Apparent viscosity and particle pressure of a concentrated suspension of non-Brownian hard spheres near the jamming transition

We consider the steady shear flow of a homogeneous and dense assembly of hard spheres suspended in a Newtonian viscous fluid. In a first part, a mean-field approach based on geometric arguments is used to determine the viscous dissipation in a dense isotropic suspension of smooth hard spheres and the hydrodynamic contribution to the suspension viscosity. In a second part, we consider the coexistence of transient solid clusters coupled to regions with free flowing particles near the jamming transition. The fraction of particles in transient clusters is derived through the Landau-Ginzburg concepts for first-order phase transition with an order parameter corresponding to the proportion of “solid” contacts. A state equation for the fraction of particle-accessible volume is introduced to derive the average normal stresses and a constitutive law that relates the total shear stress to the shear rate. The analytical expression of the average normal stresses well accounts for numerical or experimental evaluation of the particle pressure and non-equilibrium osmotic pressure in a dense sheared suspension. Both the friction level between particles and the suspension dilatancy are shown to determine the singularity of the apparent shear viscosity and the flow stability near the jamming transition. The model further predicts a Newtonian behavior for a concentrated suspension of neutrally buoyant particles and no shear thinning behavior in relation with the shear liquefaction of transient solid clusters.     

Paradoxical magnetic cooling in a structural transition model

In contrast to the experimentally widely used isentropic demagnetization process for cooling to ultra-low temperatures we examine a particular classical model system that does not cool, but rather heats up with isentropic demagnetization. This system consists of several magnetite particles in a colloidal suspension, and shows the uncommon behavior of disordering structurally while ordering magnetically in an increasing magnetic field. For a six-particle system, we report an uncommon structural transition from a ring to a chain as a function of magnetic field and temperature. Received 5 September 2000     

How a liquid becomes a glass both on cooling and on heating

The onset of structural arrest and glass formation in a concentrated suspension of silica nanoparticles in a water-lutidine binary mixture near its consolute point is studied by exploiting the near-critical fluid degrees of freedom to control the strength of an attraction between particles and multispeckle x-ray photon correlation spectroscopy to determine the particles' collective dynamics. This model system undergoes a glass transition both on cooling and on heating, and the intermediate liquid realizes unusual logarithmic relaxations. How vitrification occurs for the two different glass transitions is characterized in detail and comparisons are drawn to recent theoretical predictions for glass formation in systems with attractive interactions.     

Experimental verification of rapid, sporadic particle motions by direct imaging of glassy colloidal systems

We analyze data from confocal microscopy experiments of a colloidal suspension to validate predictions of rapid sporadic events responsible for structural relaxation in a glassy sample. The trajectories of several thousand colloidal particles are analyzed, confirming the existence of such rapid events responsible for the structural relaxation of significant regions of the sample, and complementing prior observations of dynamical heterogeneity. Thus, our results provide the first direct experimental verification of the emergence of relatively compact clusters of mobility which allow the dynamics to transition between the large periods of local confinement within its potential energy surface, in good agreement with the picture envisioned long ago by Adam and Gibbs and Goldstein.     

Fouling dynamics in suspension flows

A particle suspension flowing in a channel in which fouling layers are allowed to form on the channel walls is investigated by numerical simulation. A two-dimensional phase diagram with at least four different behaviors is constructed. The fouling is modeled by attachment during collision with the deposits and by detachment caused by large enough hydrodynamic drag. For fixed total number of particles and small Reynolds numbers, the relevant parameters governing the fouling dynamics are the solid volume fraction of the suspension and the detachment drag force threshold. Below a critical curve in this 2D phase space only transient fouling takes place when the suspension is accelerated from rest by a pressure gradient. Above the fouling transition line, persistent fouling layers are formed via ballistic deposition for low and via homogeneous deposition for large solid volume fractions. Close to the fouling transition line, the flow path between the deposited layers meanders, while necking appears for increasing distance from the transition. Finally, another transition to a fully blocked flow path takes place. As determined by the estimated amount of deposited particles at saturation, both transitions seem to be discontinuous. Large fluctuations and long saturation times are typical of the dynamics of the system.     

Nature of an electric-field-induced colloidal martensitic transition

We study the properties of a solid-solid close-packed to body-centered tetragonal transition in a colloidal suspension via fluorescence confocal laser scanning microscopy, in three dimensions and in real space. This structural transformation is driven by a subtle competition between gravitational and electric dipolar field energy, the latter being systematically varied via an external electric field. The transition threshold depends on the local depth in the colloidal sediment. Structures with order intermediate between close-packed and body-centered tetragonal were observed, with these intermediate structures also being stable and long lived. This is essentially a colloidal analogue of an "atomic-level" interfacial structure. We find qualitative agreement with theory (based purely on energetics). Quantitative differences can be attributed to the importance of entropic effects.     

Particle-like and fluid-like settling of a stratified suspension

The gravitational settling of inhomogeneously suspended particles in a fluid has been investigated. Of particular interest is whether collective or individual motion of particles is dominant during their settlings, i.e., whether the particles settle as a continuous suspension or they settle individually relative to the surrounding fluid. We observed the settling of a stratified suspension which has the lower and upper concentration interfaces in a quasi-two-dimensional vessel. In some cases, the suspension behaves perfectly as a continuous fluid and the motion of the constituent particle is subject to bulk flow caused by the interfacial instability. In other cases, the particle behaves individually relative to the surrounding fluid. The existence of a concentration interface plays a significant role in these extreme behaviors of suspension. The transition from the collective to individual behaviors can be predicted quantitatively by a parameter which expresses the border resolution of the concentration interface.     

Dilatant flow of concentrated suspensions of rough particles

The flow anisotropy of a concentrated colloidal suspension at the jamming transition is studied. It is shown that the use of rough spherical particles reduces the hydrodynamic lubrication forces between adjacent colloids and makes possible the study of the stress tensor anisotropy. At low shear rates, the suspension exerts an attractive force between two opposite surfaces, whereas at higher shear rates it becomes dilatant. Direct confocal microscopy observation of the particles organization reveal that crystallites form at high shear rate.     

Zr纳米粒子内HCP-BCC堆积结构转变的分子动力学模拟

本文采用基于嵌入原子势的分子动力学方法模拟了不同粒径的Zr纳米粒子在升温过程中HCP-BCC结构转变的路径。通过对粒子在升温过程中的势能差分曲线的计算,分别确定了小粒径、较大粒径和大粒径粒子的结构转变温度区间,并使用二分法进一步确定了转变温度点。然后借助对结构转变温度点处的形状因子、键对占比和原子堆积结构随弛豫时间的变化的模拟计算,确定了驰豫过程中堆积结构的演变过程。计算结果表明,小粒径粒子存在着多个结构转变温度点,并会在较低的结构转变温度点处出现多结构共存现象,其驰豫过程就是不同结构间相互竞争的过程。随着粒径的增大,在较高温度点处虽然仍会出现多结构共存,但粒子内的大部分原子堆积为BCC结构,并且在大粒径粒子内会出现明显的界面区。     

Bistability and "negative" viscosity for a suspension of insulating particles in an electric field

It is shown that a suspension of insulating particles in a liquid with low conductivity possesses bistability and has a "negative" effective viscosity effect in the electric field due to internal rotations. By Brownian dynamics simulation it has been found that thermal fluctuations of the angular velocity of particles in this bistable system can have a large effect on the viscosity of the suspension.     

Temperature dependence of the critical magnetic field of the structural transition in MBBA-based ferronematics

We studied the structural transitions in ferronematics based on the thermotropic nematic liquid crystal MBBA (4^′ -methoxybenzylidene-4-n-butylaniline) having a nematic-to-isotropic transition temperature T _N–I?=?48.0^○C and in MBBA-based ferronematics doped with a magnetic suspension consisting of Fe₃O₄ particles (10?nm in diameter) coated with oleic acid as a surfactant. The ferronematic samples were prepared with different volume concentrations of magnetic particles φ?=,1× 10^?4, 2× 10^?4 and 5×10^?4. The temperature dependences of the critical magnetic fields in a bias electric field under strong applied magnetic fields are presented. We calculated the surface density of anchoring energy W at the nematic–magnetic particle boundary. Scaling of the structural transition in the MBBA and MBBA-based ferronematics with the temperature of the nematic-to-isotropic transition was observed.     

Temperature-induced particle self-assembly

Agglomeration of monodisperse thiol-stabilized gold particles with diameters of 6 nm, suspended in organic solvents, was induced by the cooling of the suspension. A sharp transition between the stable suspension and agglomeration resulted. The temperature of the transition depends on the concentration and the compatibility of the solvent. The morphology of the formed particle structures upon agglomeration implies that the used metal colloid can be described as a van der Waals-gas. The particles undergo phase transitions from a stable fluid phase to a metastable phase, in which nucleation and growth occur, or to an instable phase, in which spinodal decomposition occurs. The results will direct research on routes to nanostructured materials using nanoparticles as building blocks.     

Two scenarios for colloidal phase transitions

A two-dimensional assembly of charged colloidal particles induced by an alternating electric field was studied in real space by means of digital video microscopy. Phase transitions occur from a highly ordered colloidal monolayer to an isotropic suspension by changing the field strength or frequency (in the appropriate range). In particular, it is found that the strength-dependent phase transition is an infinite-order phase transition, in contrast with the frequency-dependent phase transition, which is a second-order phase transition.     

Diagnostics of plasmon resonance in optical absorption spectra of nanographite aqueous suspensions

A characteristic feature near ～255 nm has been revealed in the optical absorption spectra of nano-graphite aqueous suspensions. This is a broad absorption peak, which is due to the surface plasmon resonance in nanographite particles. The peak shape and intensity depend on the structural quality and aggregate state of onion-like nanographite particles in suspension.     

New electric-field-driven mesoscale phase transitions in polarized suspensions

We report the discovery of a new class of an electric field-driven bulk phase transition due solely to dipolar interactions in a suspension under the action of a uniform ac field where the effects of other competing forces are suppressed. This transition appears after the well-known chain-column formation and causes the uniform suspension of columns to rearrange into a cellular pattern consisting of particle-free domains surrounded by particle-rich walls. Interestingly, the characteristic size of these domains scales linearly with the interelectrode spacing and remains insensitive to the size of the particles.